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Rare earth element-doped perovskite-type Ru-loading ammonia-synthesis catalyst

A rare earth element and perovskite type technology, which is applied in the direction of catalyst carrier, physical/chemical process catalyst, metal/metal oxide/metal hydroxide catalyst, etc., can solve the problem of no industrial promotion and application value, low ammonia synthesis activity, Reduce the problems of catalyst stability and life, and achieve the effects of inhibiting hydrogen adsorption, reducing the amount of precious metals, and improving the activity of low-temperature and low-pressure ammonia synthesis

Inactive Publication Date: 2013-10-23
FUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the contact between carbon materials and ruthenium makes methanation reaction prone to occur under ammonia synthesis conditions, which reduces the stability and life of the catalyst, thus adversely affecting the industrial application of ruthenium catalysts.
Therefore, the preparation of highly active ruthenium-based ammonia synthesis catalysts using highly stable oxide materials instead of activated carbon as a carrier has become a research hotspot in this field; the common oxide carriers in the field of ruthenium-based ammonia synthesis catalysts are mainly Al 2 o 3 , MgO, rare earth oxides and other porous nanomaterials have low ammonia synthesis activity under low temperature and low pressure conditions, and have no industrial application value

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0041] Ba(NO 3 ) 2 : Zr(NO 3 ) 4 . 5H 2 O: Y(NO 3 ) 3 . 6H 2 O: The mixture with the molar ratio of citric acid 1:0.9:0.1:3.0 was dissolved in an appropriate amount of distilled water to obtain a colorless clear viscous liquid. The solution was slowly heated in a water bath at 80°C for 4 h to evaporate excess water, and then heated at a constant temperature of 90°C for 12 h to promote the gelation of the mixture. Finally, the obtained yellow gel was calcined at 300 °C for 1 h to obtain the precursor, and then calcined at 1000 °C for 10 h to obtain the BaZr 0.9 Y 0.1 o 2.95 carrier material. The active component ruthenium was impregnated into the carrier by equal volume impregnation method, and then reduced with absolute ethanol. The active component Ru accounted for 2% of the mass fraction of the carrier. The catalyst is at 3 MPa with a space velocity of 10000 h -1 At 350°C, 375°C, 400°C and 425°C, the outlet ammonia concentrations were 2.42%, 5.80%, 7.86% and 7....

Embodiment 2

[0043] Catalyst preparation method is the same as embodiment 1, but BaZr 0.9 Y 0.1 o 2.95 The calcination temperature of the precursor is 800°C, and other conditions are the same. Get BaZr 0.9 Y 0.1 o 2.95 The specific surface area is 9.97m 2 .g -1 , the ruthenium catalyst was obtained by equal volume impregnation method. At 3 MPa, the air velocity is 10000 h -1 At 350°C, 375°C, 400°C and 425°C, the outlet ammonia concentrations were 2.13%, 4.72%, 7.03% and 7.69%, respectively.

Embodiment 3

[0045] Catalyst preparation method is the same as embodiment 1, but BaZr 0.9 Y 0.1 o 2.95 The calcination temperature of the precursor is 1100°C, and other conditions are the same. Get BaZr 0.9 Y 0.1 o 2.95 The specific surface area is 6.69m 2 .g -1 , the ruthenium catalyst was obtained by equal volume impregnation method. At 3 MPa, the air velocity is 10000 h -1 At 350°C, 375°C, 400°C and 425°C, the outlet ammonia concentrations were 0.46%, 0.92%, 2.06% and 4.15%, respectively.

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Abstract

The invention discloses a rare earth element-doped BaZrO3-delta-based perovskite-type Ru-loading ammonia-synthesis catalyst and a preparation method thereof. The rare earth element-doped BaZrO3-delta-based perovskite-type Ru-loading ammonia-synthesis catalyst utilizes a rare earth element-doped BaZrO3-delta-based perovskite-type composite oxide as a carrier having a molecular formula of Ba1-xLnx+yZr1-yO3-delta and comprises Ru as an active component. A rare earth element doping amount is 1-20wt% of the total amount of the carrier. K2RuO4 is utilized as a precursor of the active component and is directly dipped into the carrier, wherein the Ru loading amount is 0.5-10wt% of the carrier amount. The preparation method has simple processes, adopts simple equipment, does not need an auxiliary agent, and has a low precious metal use amount. The rare earth element-doped BaZrO3-delta-based perovskite-type Ru-loading ammonia-synthesis catalyst has good low-temperature low-pressure activity and high stability.

Description

technical field [0001] The invention relates to a BaZrO doped with rare earth elements, which takes metal ruthenium as the active component 3-δ The invention discloses an ammonia synthesis catalyst and a preparation method of a perovskite-based carrier loaded with ruthenium, which belong to the technical field of fertilizer catalysts and are applied to the synthesis of ammonia from a mixture of hydrogen and nitrogen. Background technique [0002] The ruthenium-based ammonia synthesis catalyst is known as the second-generation ammonia synthesis catalyst after the molten iron catalyst, and has the characteristics of low temperature, low pressure and high activity. Among them, the ruthenium-based ammonia synthesis catalyst supported by graphitized activated carbon materials has achieved industrial application in the 1990s. Chinese patents CN101362080A and CN101053834A disclose an ammonia synthesis catalyst with ruthenium as an active component, activated carbon as a carrier, a...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/63B01J32/00C01C1/04
CPCY02P20/52
Inventor 林建新马运翠王自庆倪军林炳裕魏可镁
Owner FUZHOU UNIV
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